基于MXene衍生MoS2/TiO2/Ti3C2纳米线的乳酸光重整并同步产氢

doi:10.1016/S1872-2067(24)60244-5

催化学报 ›› 2025, Vol. 71: 234-245.DOI: 10.1016/S1872-2067(24)60244-5

基于MXene衍生MoS₂/TiO₂/Ti₃C₂纳米线的乳酸光重整并同步产氢

Seemal Mansoor^a, 胡子旭^b, 张雨欣^b, Muhammad Tayyab^e, Mazhar Khan^a, Zeeshan Akmal^a, 周亮^b^,^c^,^d^,^*(), 雷菊英^b^,^d, Muhammad Nasir^f, 张金龙^a^,^*()

^a华东理工大学化学与分子工程学院, 先进材料重点实验室, 上海多介质环境催化与资源化工程技术研究中心, 国际精细联合研究实验室, 费林加诺贝尔奖科学家联合研究中心, 上海 200237, 中国
^b华东理工大学资源与环境工程学院, 工业废水无害化与资源化国家工程研究中心, 生态环境部化工过程环境风险评价与控制重点实验室, 上海 200237, 中国
^c哈尔滨工业大学, 城市水资源与水环境国家重点实验室, 黑龙江哈尔滨 150090, 中国
^d上海污染控制与生态安全研究院, 上海 200092, 中国
^e清华大学深圳国际研究生院, 广东深圳 518055, 中国
^fCOMSATS大学伊斯兰堡分校, 生物医学材料跨学科研究中心, 拉合尔, 巴基斯坦

收稿日期:2024-11-14 接受日期:2024-12-20 出版日期:2025-04-18 发布日期:2025-04-13
通讯作者: * 电子信箱: zhouliang@ecust.edu.cn (周亮), jlzhang@ecust.edu.cn (张金龙).
基金资助:
国家重点研发项目(2022YFB3803600);国家重点研发项目(2022YFE0107900);国家自然科学基金(22476050);国家自然科学基金(21972040);上海市教委创新计划(2021-01-07-00-02-E00106);上海市科学技术委员会(22230780200);上海市科学技术委员会(20DZ2250400);中央高校基本科研业务费(222201717003);城市水资源与水环境国家重点实验室开放课题(QA202319);上海市教委晨光项目(23CGA40)

Simultaneous hydrogen production with photo reforming of lactic acid over MXene derived MoS₂/TiO₂/Ti₃C₂ nanowires

Seemal Mansoor^a, Zixu Hu^b, Yuxin Zhang^b, Muhammad Tayyab^e, Mazhar Khan^a, Zeeshan Akmal^a, Liang Zhou^b^,^c^,^d^,^*(), Juying Lei^b^,^d, Muhammad Nasir^f, Jinlong Zhang^a^,^*()

^aKey Laboratory for Advanced Materials, Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science & Technology, Shanghai 200237, China
^bNational Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery, State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai 200237, China
^cState Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, Heilongjiang, China
^dShanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
^eInstitute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, Guangdong, China
^fCOMSATS Univ Islamabad, Interdisciplinary Res Ctr Biomed Mat IRCBM, Lahore Campus, Lahore 54000, Pakistan

Received:2024-11-14 Accepted:2024-12-20 Online:2025-04-18 Published:2025-04-13
Contact: * E-mail: zhouliang@ecust.edu.cn (L. Zhou),jlzhang@ecust.edu.cn (J. Zhang).
Supported by:
National Key Research and Development Program of China(2022YFB3803600);National Key Research and Development Program of China(2022YFE0107900);National Natural Science Foundation of China(22476050);National Natural Science Foundation of China(21972040);Innovation Program of Shanghai Municipal Education Commission(2021-01-07-00-02-E00106);Science and Technology Commission of Shanghai Municipality(22230780200);Science and Technology Commission of Shanghai Municipality(20DZ2250400);Fundamental Research Funds for the Central Universities(222201717003);Open Project of State Key Laboratory of Urban Water Resource and Environment(QA202319);Chenguang Program of Shanghai Education Development Foundation, and the Shanghai Municipal Education Commission(23CGA40)

摘要/Abstract

摘要：

聚乳酸(PLA)作为一种可降解塑料, 已被广泛应用于市场. 光催化技术作为一种绿色、可持续的处理方法, 在PLA资源化转化方面展现出显著潜力. 尽管前期研究主要集中在光催化产氢和增值化合物的合成上以应对能源和环境危机. 当前研究趋势正转向通过光重整技术实现塑料氧化过程调控, 不仅解决有害化合物污染问题, 并生成绿色能源. 该反应的关键在于有序地打破乳酸中的C-OH和C-H键, 构健PLA到丙酮酸(PA)的高选择性回收路径. 因此, 设计高性能的光催化剂, 成为实现PLA向PA高选择性定向转化的关键科学挑战.
本文设计了一种高效的MoS₂/TiO₂/Ti₃C₂纳米线光催化系统, 在紫外-可见光照射下, 实现了PLA的氧化转化并生成氢气. 首先, Ti₃C₂纳米片被转化为TiO₂/Ti₃C₂ (TTC)纳米线复合材料, 随后通过水热过程将MoS₂均匀负载在TTC复合材料表面, 产生协同效应以提高光催化剂的活性. 在光催化产氢测试中, 以三乙醇胺作为牺牲试剂, 获得的最高的氢气产生速率为637.1 μmol g^{- 1} h^-1, 是TTC纳米线的7.1倍. 进一步拓展该体系至PLA转化体系, 使用预处理的PLA溶液作为牺牲试剂时, 氢气产生速率为243.2 μmol g^-1 h^-1, 并同步实现了PLA向PA的选择性氧化转化. Ti₃C₂和MoS₂的结合形成了有效的复合材料, 因双助催化剂的协同效应而增强了光催化活性. 将MoS₂加入TTC光催化剂中, 提高了氢气生成的特定活性(请重新梳理此句表达). PLA塑料在光照下解聚为乳酸, 乳酸通过空穴氧化为丙酮酸离子, 这些丙酮酸离子进一步转化为PA, 最终实现了PLA塑料直接光重整和氢气生成.
综上, 本文以原位生成和后负载两种方式制备了双助光催化剂, 在光照下同步实现了废弃塑料的资源化与产氢, 极大地提高了光催化技术经济价值, 为后续相关高价值体系的开发和应用提供参考.

关键词: 光重整, 聚乳酸, 析氢, 乳酸, 丙酮酸

Abstract:

Developing efficient photocatalysts to address collaborative energy and environmental crises still faces significant challenges. In this report, we present a highly efficient MXene-based photocatalyst, which is combined with MoS₂ nano patches and TiO₂/Ti₃C₂ (TTC) nanowires through hydrothermal treatment. Of all the composites tested, the optimized photocatalyst gave a remarkable H₂ and revolving polylactic acid (PLA) into pyruvic acid (PA). Achieving a remarkable H₂ evolution rate of 637.1 and 243.2 μmol g⁻¹ h⁻¹, in the presence of TEOA and PLA as a sacrificial reagent under UV-vis (λ ≥ 365 nm) light irradiation. The improved photocatalytic activity is a result of the combination of dual cocatalyst on the surface of TTC photocatalyst, which create an ideal synergistic effect for the generation of PA and the production of H₂simultaneously. The MoS₂TiO₂/Ti₃C₂ (MTT) composite can generate more photoexcited charge carriers, leading to the generation of more active radicals, which may enhance the system's photocatalytic activity. This work aims at demonstrating its future significance and guide the scientific community towards a more efficient approach to commercializing H₂ through photocatalysis.

Key words: Photo reforming, Polylactic acid, Hydrogen evolution, Lactic acid, Pyruvic acid

Seemal Mansoor, 胡子旭, 张雨欣, Muhammad Tayyab, Mazhar Khan, Zeeshan Akmal, 周亮, 雷菊英, Muhammad Nasir, 张金龙. 基于MXene衍生MoS₂/TiO₂/Ti₃C₂纳米线的乳酸光重整并同步产氢[J]. 催化学报, 2025, 71: 234-245.

Seemal Mansoor, Zixu Hu, Yuxin Zhang, Muhammad Tayyab, Mazhar Khan, Zeeshan Akmal, Liang Zhou, Juying Lei, Muhammad Nasir, Jinlong Zhang. Simultaneous hydrogen production with photo reforming of lactic acid over MXene derived MoS₂/TiO₂/Ti₃C₂ nanowires[J]. Chinese Journal of Catalysis, 2025, 71: 234-245.

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图/表 8

Fig. 1. Schematic illustration of the MTT nanowires photocatalyst.

Fig. 2. (a-c) SEM images of Ti3C2, TTC, MTT-2. (d,e) TEM images of TTC and MTT-2. HRTEM analysis (f,g) and d-spacing (h-j) of TiO2, Ti3C2, MoS2 in MTT-2.

Fig. 3. HAADF-STEM image (a) and elemental mapping of Ti (b), O (c), Mo (d), S (e), and C (f) of MTT-2 photocatalyst.

Fig. 4. (a) XRD patterns Ti3AlC2, Ti3C2, TTC, TOTC, different concentrations of MTT, and pristine MoS2. (b) FTIR spectra of TTC and MTT-2. (c) Raman spectra of MTT-2, TTC, TOTC.

Fig. 5. XPS full spectra(a), high resolution XPS spectra of O 1s (b), Ti 2p (c), and C 1s (d) in Ti3C2, TTC and MTT-2 photocatalyst.

Fig. 6. H2 evolution activity test of representative photocatalysts in the presence of TEOA as a hole scavenger (a) and in the presence of PLA (b). Note: the error bar is estimated from the average value of three repeated experiments. Long time cyclic stability test in TEOA (c) and in the PLA (d) of MTT-2 photocatalyst. (e) Schematic illustration of the photo reforming process of PLA into PA. (f) Comparison of photocatalytic H2 evolution.

Fig. 7. Photoelectrochemical analysis. UV-vis DRS (a) and steady-state PL spectra (b) for representative photocatalysts. (c) Transient photocurrent responses of Ti3C2, TTC, and MTT-2. (d) Time-resolved PL spectra for TOTC, TTC, and MTT-2.

Fig. 8. EPR spectra for DMPO-?O2- (a) and DMPO-?OH (b) for TTC and MTT-2. (c) Proposed mechanism of H2 evolution and PLA oxidation over MTT nanowires.

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基于MXene衍生MoS₂/TiO₂/Ti₃C₂纳米线的乳酸光重整并同步产氢

Simultaneous hydrogen production with photo reforming of lactic acid over MXene derived MoS₂/TiO₂/Ti₃C₂ nanowires

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